Cross-shelf processes of terrigenous organic matter drive mercury speciation on the east siberian shelf in the Arctic Ocean.

The cross-shelf distributions of total mercury (THg), methylmercury (MeHg) and organic and inorganic matter, as well as the presence of the hgcA gene were investigated on the East Siberian Shelf (ESS) to understand the processes underlying the speciation of sedimentary Hg. Samples were collected from 12 stations grouped into four zones based on water depth: inner shelf (5 stations), mid-shelf (3 stations), outer shelf (2 stations), and slope (2 stations). The THg concentration in the surface sediment increased from the inner shelf (0.25 ± 0.023 nmol g-1) toward the slope (0.52 nmol g-1), and, when normalized to total organic carbon content, the THg showed a positive correlation with the clay-to-sand ratio (r2 = 0.48, p = 0.012) and degree of chemical weathering (r2 = 0.79, p = 0.0001). The highest MeHg concentrations (3.0 ± 1.8 pmol g-1), as well as peaks in the S/C ratio (0.012 ± 0.002) of sediment-leached organic matter, were found on the mid-shelf, suggesting that the activities of sulfate reducers control the net Hg(II) methylation rates in the sediment. This was supported by results from a principal component analysis (PCA) performed with Hg species concentrations and sediment-leached organic matter compositions. The site-specific variation in MeHg showed the highest similarity with that of CHONS compounds in the PCA, where Deltaproteobacteria were projected to be putative Hg(II) methylators in the gene analysis. In summary, the hydrodynamic sorting of lithogenic particles appears to govern the cross-shelf distribution of THg, and in situ methylation is considered a major source of MeHg in the ESS sediment.

Metalloenzyme signatures in authigenic carbonates from the Chukchi Borderlands in the western Arctic Ocean.

Migration of methane-rich fluids at submarine cold seeps drives intense microbial activity and precipitation of authigenic carbonates. In this study, we analyzed microbially derived authigenic carbonate samples recently recovered from active gas hydrate mounds on the southwestern slope of the Chukchi Borderlands (CB), western Arctic Ocean. Our main aim was to characterize the distribution patterns of trace elements in carbonate-hosted lipid fractions to assess metalloenzyme requirements of microbes involved in anaerobic oxidation of methane (AOM). We measured stable isotopes, trace elements, lipid biomarkers, and genomic DNA, and results indicate the dominance of AOM-related lipid biomarkers in studied carbonate samples, as well as a predominant occurrence of the anaerobic methanotrophic archaea (ANME)-1. We also report evidence for significant preferential enrichments of various trace elements (Li, Ni, Co, Cu, Zn, and Mo) in the total lipid fractions of CB carbonates, relative to elemental compositions determined for corresponding carbonate fractions, which differ from those previously reported for other seep sites. We hypothesize that trace element enrichments in carbonate-hosted lipid fractions could vary depending on the type of AOM microbial assemblage. Additional work is required to further investigate the mechanisms of lipid-bound trace elements in cold seep carbonates as potential metalloenzymes in AOM.

Rapid seafloor changes associated with the degradation of Arctic submarine permafrost.

SignificanceTemperature increases in Arctic regions have focused attention on permafrost degradation on land, whereas little is known about the dynamics of extensive glacial-age permafrost bodies now submerged under the vast Arctic Continental shelves. Repeated high-resolution bathymetric surveys show that extraordinarily rapid morphologic changes are occurring at the edge of the continental slope of the Canadian Beaufort Sea along what was once the seaward limit of relict Pleistocene permafrost. How widespread similar changes are on the Arctic shelves is unknown, as this is one of the first areas in the Arctic subjected to multiple multibeam bathymetric surveys. Rapid morphologic changes associated with active submarine permafrost thawing may be an important process in sculpturing the seafloor in other submarine permafrost settings.

Hymenobacter siberiensis sp. nov., isolated from a marine sediment of the East Siberian Sea and Hymenobacter psoromatis sp. nov., isolated from an Antarctic lichen.

Gram-stain-negative, strictly aerobic, red-pink-coloured, rod-shaped and non-motile bacterial strains PAMC 29290, PAMC 29294T and PAMC 29296 were isolated from marine surface sediment sampled in the East Siberian Sea and strains PAMC 26553 and PAMC 26554T were obtained from an Antarctic lichen. Strains PAMC 29290, PAMC 29294T and PAMC 29296 were closely related to Hymenobacter artigasi (98.8 % 16S rRNA gene similarity), Hymenobacter antarcticus (97.3 %) and Hymenobacter glaciei (96.9 %), and PAMC 26553 and PAMC 26554T showed high similarity to Hymenobacter ginsengisoli (97.0 %), Hymenobacter rivuli (96.1 %) and Hymenobacter setariae (95.9 %). Genomic relatedness analyses showed that strains PAMC 29290, PAMC 29294T and PAMC 29296 could be distinguished from H. artigasi by average nucleotide identity (ANI; 93.1-93.2 %) and digital DNA-DNA hybridization (dDDH; 50.3-51.0 %) values. Strains PAMC 26553 and PAMC 26554T could be clearly distinguished from H. ginsengisoli with ANI values <79.8 % and dDDH values <23.3 %. The major fatty acids of strains PAMC 29290, PAMC 29294T and PAMC 29296 were C15 : 0 iso (21.0-26.0 %), summed feature 3 (C16 : 1 ω7c and/or C16 : 1 ω6c; 17.4-18.2 %), C15 : 0 anteiso (12.7-19.1 %) and summed feature 4 (C17 : 1 iso I and/or anteiso B; 8.6-16.1 %) and those of strains PAMC 26553 and PAMC 26554T were summed feature 3 (C16 : 1 ω7c and/or C16 : 1 ω6c; 20.7-22.2 %), C15 : 0 anteiso (17.5-19.7 %) and summed feature 4 (C17 : 1 iso I and/or anteiso B; 15.5-18.1 %). The major respiratory quinone was MK-7. The genomic DNA G+C contents were 60.6-60.8 mol%. The polar lipids of PAMC 29294T were found to consist of phosphatidylethanolamine, four unidentified aminolipids, an unidentified aminophospholipid and five unidentified lipids; those of PAMC 26554T were phosphatidylethanolamine, three unidentified aminolipids, four unidentified aminophospholipid and two unidentified lipids. The distinct phylogenetic position and some physiological characteristics distinguished the novel strains from closely related type strains in the genus Hymenobacter. Thus, two novel species are proposed, with the names Hymenobacter siberiensis sp. nov. (type strain, PAMC 29294T=KCTC 82466T=JCM 34574T) and Hymenobacter psoromatis sp. nov. (type strain, PAMC 26554T=KCTC 82464T=JCM 34572T), respectively.

The impact of the abnormal salinity enrichment in pore water on the thermodynamic stability of marine natural gas hydrates in the Arctic region.

In this study, the thermodynamic and structural characteristics of natural gas hydrates (NGHs) retrieved from gas hydrate mounds (ARAON Mound 03 (AM03) and ARAON Mound 06 (AM06)) in the Chukchi Sea in the Arctic region were investigated. The gas compositions, crystalline structure, and cage occupancy of the NGHs at AM03 and AM06 were experimentally measured using gas chromatography (GC), 13C nuclear magnetic resonance (NMR), Raman spectroscopy, and powder X-ray diffraction (PXRD). In the NGHs from AM03 and AM06, a significantly large fraction of CH4 (> 99%) and a very small amount of H2S were enclathrated in small (512) and large (51262) cages of sI hydrate. The NGHs from AM03 and AM06 were almost identical in composition, guest distributions, and existing environment to each other. The salinity of the residual pore water in the hydrate-bearing sediment (AM06) was measured to be 50.32‰, which was much higher than that of seawater (34.88‰). This abnormal salinity enrichment in the pore water of the low-permeability sediment might induce the dissociation of NGHs at a lower temperature than expected. The saturation changes in the NGHs that corresponded with an increase in the seawater temperature were also predicted on the basis of the salinity changes in the pore water. The experimental and predicted results of this study would be helpful for understanding the thermodynamic stability of NGHs and potential CH4-releasing phenomena in the Arctic region.

Subsea permafrost as a potential major source of dissolved organic matter to the East Siberian Arctic Shelf.

Arctic subsea permafrost contains more organic carbon than the terrestrial counterpart (~1400 Pg C vs. ~1000 Pg C) and is undergoing fast degradation (at rates of ~10 to 30 cm yr-1 over the past 3 decades) in response to climate warming. Yet the flux of organic carbon sequestered in the sediments of subsea permafrost to overlying water column, which can trigger enormous positive carbon-climate feedbacks, remain unclear. In this study, we examined the dissolved organic matter (DOM) diffusion to bottom seawaters from East Siberian Sea (ESS) sediments, which was estimated at about 943-2240 g C m-2 yr-1 and 10-55 g C m-2 yr-1 at the continuous-discontinuous transition zone of subsea permafrost and the remainder shelf and slope sites, respectively. The released DOM is characterized by prevailing dominance (≥ 98%) of low molecular weight (Mn < 350 Da) fractions. A red-shifted (emission wavelength >500 nm) fluorescence fingerprint, a typical feature of sediment/soil DOM, accounts for 4-6% and 7-8% in the fluorescence distributions of seawaters and pore waters, respectively, on ESS shelf. Statistical analysis revealed that seawaters and pore waters possessed similar DOM composition. The estimated total benthic efflux of dissolved organic carbon (DOC) was ~0.7-1.0 Pg C yr-1 when the estimate was scaled up to the entire Arctic shelf underlain with subsea permafrost assuming the width of continuous-discontinuous transition zone is 1 to 10 m. This estimation is consistent with the established ~10-30 cm yr-1 degradation rates of subsea permafrost by estimating its thaw-out time. Compiled observation data suggested that subsea permafrost might be a major DOM source to the Arctic Ocean, which could release tremendous carbon upon remineralization via its degradation to CO2 and CH4 in the water column.

Mass Budget of Methylmercury in the East Siberian Sea: The Importance of Sediment Sources.

Biological concentrations of methylmercury (MeHg) are elevated throughout the Arctic Ocean; however, to date, the major sources and the spatial variability of MeHg are not well quantified. To identify the major inputs and outputs of MeHg to the Arctic shelf water column, we measured MeHg concentrations in the seawater and sediment samples from the East Siberian Sea collected from August to September 2018. We found that the MeHg concentrations in seawater and pore water were higher on the slope than on the shelf, while the MeHg concentrations in the sediment were higher on the shelf than on the slope. We created a mass budget for MeHg and found that the benthic diffusion and resuspension largely exceed other sources, such as atmospheric deposition and river water input. The major sinks of MeHg in the water column were dark demethylation and evasion. When we extrapolated our findings on benthic diffusion to the entire Arctic shelf system, the annual MeHg diffusion from the shelf sediments was estimated to be 23,065 ± 939 mol yr-1, about 2 times higher than previously proposed river discharges. Our study suggests that the MeHg input from shelf sediments in the Arctic Ocean is significant and has been previously underestimated.

Antarcticibacterium arcticum sp. nov., a bacterium isolated from marine sediment of the Canadian Beaufort Sea.

A Gram-stain-negative, aerobic, yellow-pigmented, flexirubin-negative, rod-shaped and non-motile bacterial strain, PAMC 28998T, was isolated from a surface sediment sample collected from the Canadian Beaufort Sea. Strain PAMC 28998T grew at 4-37 °C (optimum, 25 °C), at pH 7.0-9.0 (optimum, pH 7.5) and in the presence of 1.0-10.0 % (w/v) NaCl. Phylogenetic analysis based on the 16S rRNA gene sequence revealed that strain PAMC 28998T belongs to the genus Antarcticibacterium showing the highest sequence similarity (96.8 %) with Antarcticibacterium flavum JB01H24T. The average nucleotide identity and genome-to-genome distance values between PAMC 28998T and the most closely related species (A. flavum JB01H24T) were 74.1 and 18.5 %, respectively, indicating that strain PAMC 28998T is clearly distinguished from A. flavum. The genomic DNA G+C content calculated from genome sequences was 39.8 %. The major fatty acids (>10 %) were iso-C15 : 0 (19.5 %), anteiso-C15 : 0 (18.0 %), iso-C16 : 0 (11.6 %) and summed feature 3 (C16:1 ω6c and/or C16:1 ω7c; 11.4 %). The major polar lipids were phosphatidylethanolamine, aminoglycolipid, two unidentified aminolipids, three unidentified phospholipids and four unidentified lipids. The major respiratory quinone was MK-6. Based on the phylogenetic, genomic and phenotypic data presented here, strain PAMC 28998T is considered to represent a novel species of the genus Antarcticibacterium, for which the name Antarcticibacterium arcticum sp. nov. is proposed with the strain PAMC 28998T (=KCCM 43316 T=JCM 33514T).

Discriminative biogeochemical signatures of methanotrophs in different chemosynthetic habitats at an active mud volcano in the Canadian Beaufort Sea.

Several mud volcanoes are active in the Canadian Beaufort Sea. In this study, we investigated vertical variations in methanotrophic communities in sediments of the mud volcano MV420 (420 m water depth) by analyzing geochemical properties, microbial lipids, and nucleic acid signatures. Three push cores were collected with a remotely operated vehicle from visually discriminative habitats that were devoid of megafauna and/microbial mats (DM) to the naked eye, covered with bacterial mats (BM), or colonized by siboglinid tubeworms (ST). All MV420 sites showed the presence of aerobic methane oxidation (MOx)- and anaerobic methane oxidation (AOM)-related lipid biomarkers (4α-methyl sterols and sn-2-hydroxyarchaeol, respectively), which were distinctly different in comparison with a reference site at which these compounds were not detected. Lipid biomarker results were in close agreement with 16S rRNA analyses, which revealed the presence of MOx-related bacteria (Methylococcales) and AOM-related archaea (ANME-2 and ANME-3) at the MV420 sites. 4α-methyl sterols derived from Methylococcales predominated in the surface layer at the BM site, which showed a moderate methane flux (0.04 mmol cm-2 y-1), while their occurrence was limited at the DM (0.06 mmol cm-2 y-1) and ST (0.01 mmol cm-2 y-1) sites. On the other hand, 13C-depleted sn-2-hydroxyarchaeol potentially derived from ANME-2 and/or ANME-3 was abundant in down-core sediments at the ST site. Our study indicates that a niche diversification within this mud volcano system has shaped distinct methanotrophic communities due to availability of electron acceptors in association with varying degrees of methane flux and bioirrigation activity.

Increase in anthropogenic mercury in marginal sea sediments of the Northwest Pacific Ocean.

Over the past century, the addition of anthropogenic mercury (HgANTH) to vast areas of North Pacific marginal seas adjacent to the northeast Asian continent has tripled. Analysis of sediment cores showed that the rate of HgANTH addition (HgANTH flux) was greatest in the East China and Yellow Seas (9.1 µg m-2 yr-1) in the vicinity of China (the source continent), but was small in the Bering and western Arctic Ocean (Chukchi Sea) (0.9 µg m-2 yr-1; the regions furthest from China). Our results show that HgANTH has reached open ocean sedimentary environments over extended areas of the northwestern Pacific Ocean, via the formation of organic-mercury complexes and deposition. The implication of these findings is that the addition of HgANTH (via atmospheric deposition and riverine input) to the ocean environment is responsible for elevated Hg flux into sedimentary environments in the northwest Pacific Ocean.